Notice of Pre-AIA or AIA Status
The present application, filed on or after March 16, 2013, is being examined under the first inventor to file provisions of the AIA .
Status of Claims
Applicant’s amendment and arguments filed 10/14/2025 have been fully considered. Claim(s) 15-22 is/are amended; claim(s) 23-28 remain withdrawn. Claims 15-22 are pending review in this Office action. Examiner affirms that the original disclosure provides adequate support for the amendment.
Upon considering said amendment and arguments, the previous rejection under 35 U.S.C. 103 set forth in the Office action mailed 07/25/2025 has been withdrawn. Applicant’s amendment necessitated the new grounds of rejection below.
Claim Rejections - 35 USC § 103
The text of those sections of Title 35, U.S. Code not included in this action can be found in a prior Office action.
Claims 15-22 are rejected under 35 U.S.C. 103 as being unpatentable over Kosuzu et al. (US20030157407A1 cited in Office action filed 07/25/2025) in view of Matsuno et al. (US20190341602A1), evidenced by University of Cambridge (“The interactive Ellingham diagram”, see copy provided with this Office action)
Regarding claim 15, 19, 20, Kosuzu discloses a silicon-based powder (“electrode material”) suitable for use in a negative electrode of a battery, the silicon-based powder comprising at least the silicon-based particles ([0020]). While Kozusu envisions the use of additives in the silicon-based powder for purposes of improving conductivity or preventing particle aggregation, ([0120-0123]), and recognizes a problem of lithium deposition on the negative electrode ([0007], [0045]), Kosuzu does not disclose the use of a non-silicon-based particle in the silicon-based powder for this purpose.
Matsuno is directed to a silicon-based powder suitable for use in a negative electrode of a battery analogously comprising silicon-based particles (Matsuno [0013-0014]), further teaching the addition of a non-silicon-based particle (“metal compound particle”) provided as a particle separate from (i.e., district from) the silicon-based particle (“negative electrode active material particle “) ([0016], [0105]), the non-silicon-based particle advantageously suppressing Li precipitation (i.e., deposition) in the battery during charging when provided into the silicon-based powder by improving dispersion of the silicon-based particles and avoiding formation of areas with low proportions of silicon-based particles ([0021], [0226]).
Thus, in seeking to resist the effects of lithium deposition in a negative electrode produced with Kosuzu’s silicon-based powder, it would be obvious before the effective filing date of the instant application for one having ordinary skill in the art to provide the silicon-based powder with non-silicon-based particles distinct from the silicon-based particles as taught by Matsuno. Such a modification would be made with a reasonable expectation of success, as Matsuno teaches the non-silicon-based particles for use with silicon-based particles analogous to those disclosed by Kosuzu (Kosuzu [0020]), and Kosuzu and Matsuno recognize the same inventive problem of preventing lithium deposition (Kosuzu [0007], Matsuno [0021]).
Modified Kosuzu further discloses maintaining the average particle size of the silicon-based particles within a range of at least 0.1 µm (100 nm) to prevent excessive surface area leading to uncontrolled oxidation (Kosuzu [0048]), and less than 0.5 µm (500 nm) to provide a suitably high coulombic efficiency ([0052]). While Kosuzu does not explicitly classify the silicon-based particles by a
number-based particle size distribution with a median ds50 value, Kosuzu’s silicon-based particles necessarily comprise at least some value of ds50, and the average particle size and ds50 are related based on the particle size distribution such that a skilled artisan optimizing an average particle size of Kosuzu’s silicon-based particles within a range of 100-500 nm would reasonably utilize at least a portion of the claimed range of ds50 (200 nm or less) between approximately 100-200 nm through routine optimization under Kosuzu’s disclosure (MPEP 2144.05 II); such an optimization would be done with a reasonable expectation of success as Kosuzu discloses a suitability of varying the average particle diameter within this range.
Modified Kosuzu further discloses the silicon-based powder has an oxygen content of at most 5% by weight to avoid uncontrolled oxidation during the production process and to provide a suitable coulombic efficiency value (Kosuzu [0060]), this value falling within the claimed range of 20% by weight or less.
While modified Kosuzu does not disclose the material of the non-silicon-based particles, Matsuno teaches the inclusion of aluminum, zirconium, and yttrium in the particles (Matsuno [0069]), where negative electrodes comprising all three elements in the non-silicon-based particles had the highest pass rate in a nail penetration test simulating Li deposition ([0215-0224], pp. 14 Table 3, [0226]) such that it would be obvious to select aluminum, zirconium, and yttrium as a material of modified Kosuzu’s non-silicon-based particles.
Zr, Al, and Y all have a Standard Gibbs free energy of formation of their oxides lower than that of SiO2 from zerovalent silicon (Al, Zr recited with this property in the instant specification pp. 5 ¶6-pp. 6 ¶1; Y evidenced by University of Cambridge, see below) such that using the elements taught by Matsuno inherently forms modified Kosuzu’s silicon-based powder comprising one or more elements M (Zr, Al, Y) from a group of metals that have a Standard Gibbs free energy of formation at a temperature T of the oxide from their zerovalent state which is lower than the Standard Gibbs free energy of formation at the same temperature T of SiO2 from zerovalent silicon between 573K≤T≤1373K as claimed.
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University of Cambridge - the Interactive Ellingham diagram
While modified Kosuzu does not explicitly disclose a content of elements M relative to a content of Si by weight, Matsuno teaches limiting the amount of Al to less than 1 wt% of the silicon-based particle weight (Matsuno [0072]) and Zr to 0.1 wt% (“1000 ppm”) ([0073]) for the purpose of maintaining electric conductivity, and providing at least 0.03 wt% Al and 0.001 wt% Zr to stabilize an electrode slurry ([0072-0073]) and to resist Li deposition ([0215-0224], pp. 14 Table 3, [0226]). Y is kept in a mass range assumed negligible for purposes of estimation (1-30 ppm by Si particle mass, [0074]).
As such, in seeking to balance considerations of Li deposition resistance while maintaining electric conductivity, it would be obvious before the effective filing date of the instant application for one having ordinary skill in the art to optimize a content of element M in the silicon-based powder within a range of about 0.031 wt% (0.03 wt% Al, 0.001 wt% Zr) to 1.1 wt% (1 wt% Al, 0.1 wt% Zr) of the content of Si by weight in the silicon-based powder, overlapping with portions of the claimed ranges (0.01%-5% of Si content, claim 15; 0.40%-5%, claim 19) between 0.01-1.1 wt% and 0.40-1.1 wt% such that a skilled artisan would have selected within the overlap through routine optimization under Matsuno’s teaching. Such a selection would be made with a reasonable expectation of success because Kosuzu and Matsuno are similarly directed to silicon-based powders and recognize the same consideration of resisting Li deposition (MPEP 2144.05 II). Furthermore, the group of one or more elements M comprises Zr (claim 20).
Kosuzu modified in view of Matsuno further discloses the one or more elements M as being present in the non-silicon-based particles (“metal compound particle”, Matsuno [0016], [0105]).
Regarding claim 16, modified Kosuzu discloses the silicon-based powder according to claim 15.
While Kosuzu does not explicitly specify the molar composition of the silicon-based particle surface layer as SiOx with 0<x<1, Kosuzu discloses that the silicon-based particle surface is at least partially oxidized (i.e., SiOx where x>0) to stabilize the silicon-based particles (Kosuzu [0158-0160]); simultaneously, Kosuzu avoids excessive particle surface oxidation to prevent undesirable reactions of silicon oxides with lithium during charging ([0160-0162]), necessarily limiting the average surface layer composition to SiOx where x<2 as no further oxidation can proceed in SiO2 where x=2.
As such, in seeking to balance stabilizing modified Kosuzu’s silicon-based particles without causing side reactions during charging, it would be obvious before the effective filing date of the instant application for one having ordinary skill in the art to optimize an average molar composition of the surface layer SiOx within a range of 0<x<2, encompassing the claimed range (0≤x<1) such that a skilled artisan would have selected within the encompassed range through routine optimization under Kosuzu’s disclosure with a reasonable expectation of success (MPEP 2144.05 II).
Regarding claim 17, modified Kosuzu discloses the silicon-based powder according to claim 15. While Kosuzu does not explicitly indicate the content of elements M in the non-silicon-based particles by weight when considered without oxygen, Matsuno indicates a preferability of using metal compounds bonded to oxygen for compatibility in an electrode slurry and to allow detection of the non-silicon-based particles in XPS spectroscopy; a finite list of suitable forms of Element M in non-silicon-based particles include oxides, phosphates, and silicates of Element M (Matsuno [0070]). The skilled artisan would need to select at least some compound of element M to form the non-silicon-based particles, with oxides of element M recognized as predictable solutions within the technical grasp of a skilled artisan that it would be obvious to routinely explore selecting oxides of element M to form the non-silicon-based particles with a reasonable expectation of success (MPEP 2143 I E).
As oxides of element M do not comprise other elements except oxygen, the content of element M as an oxide in non-silicon-based particles is appreciably close to 100% by weight, at least within the claimed range of at least 60% by weight when considering all elements except oxygen.
Regarding claim 18, modified Kosuzu discloses the silicon-based powder according to claim 15. While Kosuzu does not disclose the number-based particle size distribution (dNS50) of the non-silicon-based particles as being at most 500 nm, Matsuno teaches optimizing an average particle size of the non-silicon-based particles (“metal compound particles”) within a range of at least 0.1 µm (100 nm) to prevent impurities in the non-silicon-based particles from eluting (Matsuno [0088]) and less than 20 µm (20000 nm) to prevent Li precipitation ([0088]); an experimental example with 0.1 µm (100 nm) non-silicon-based particles is also shown with an especially high capacity retention and resistance to Li deposition (see Example 4-7, [0226], pp. 15 Table 4).
As such, in seeking to improve resistance to Li precipitation in modified Kosuzu’s silicon-based powder without eluting impurities, it would be obvious before the effective filing date of the instant application for one having ordinary skill in the art to optimize an average size of the non-silicon-based particles within a range of 100-20000 nm as taught by Matsuno, overlapping with a portion of the claimed range (at most 500 nm) between 100-500 nm such that a skilled artisan would have selected within the overlapped portion of dNS50 through routine optimization under Matsuno’s teaching with a reasonable expectation of success because Matsuno demonstrates an experimental example of the non-silicon-based particles having high capacity retention and resistance to Li deposition at an average size of 100 nm (MPEP 2144.05 II).
Regarding claim 21, modified Kosuzu discloses the silicon-based powder according to claim 15. Modified Kosuzu discloses that the silicon-based particles are made from 99.6-99.99% pure Si as a raw material prior to the oxidation treatment with respect to impurities (e.g., Ca, Al, Fe) (Kosuzu [0119]); the content of element M in the silicon-based powder ranges from about 0.031 wt% to 1.1 wt% of the content of Si by weight in the silicon-based powder (Matsuno [0072-0073], see discussion of claim 15).
As such, modified Kosuzu’s silicon-based powder, considering all elements except oxygen, comprises a Si content of at least about 98.5% (99.6% Si in the silicon-based powder - 1.1 wt% element M in non-silicon-based powder), this being within the claimed range of at least 90% by weight.
Regarding claim 22, modified Kosuzu discloses the silicon-based powder according to claim 15. While Kosuzu does not explicitly classify the silicon-based powder by a volumetric particle size distribution or specify an average primary particle size dav ranging from 17-172 nm, Kosuzu’s silicon-based powder necessarily comprises at least some value of dav. Kosuzu also discloses optimizing an average particle size of the silicon-based particles is in a range between 100-500 nm to balance considerations of particle stability and coulombic efficiency (Kosuzu [0048], [0052]; see discussion of claim 15). Given that particle size and particle volume are related measurements, it would be obvious for a skilled artisan performing the above optimization to have utilized at least a portion overlapping with the claimed range of dav (17-172 nm) between approximately 100-172 nm through routine experimentation under Kosuzu’s disclosure with a reasonable expectation of success (MPEP 2144.05 II).
Modified Kosuzu’s non-silicon-based particles comprise about only 0.01-1.1 wt% of the weight of the silicon-based powder on a basis of Element M (Matsuno [0072-0073], see discussion of claim 15); the weight of the non-silicon-based particles (and a corresponding volume of the particles) is sufficiently low relative to the silicon-based particles that the volume impact of ~1 vol% from the non-silicon-based particles is considered negligible for estimation purposes of the silicon-based powder’s dav.
Response to Arguments
The amendments to claims 16-22, i.e., all dependent claims, to start with “the” since they seek antecedent basis from a parent claim has overcome the previous objection to these claims in the Office action filed 07/25/2025; the objection is withdrawn.
Applicant’s arguments with respect to rejection of claim(s) 15-22 as unpatentable over Kawakami et al. (US20090162750A1), Kosuzu (US20030157407A1), evidenced by Onur (“Development of rare earth-free negative electrode materials for Ni/MH batteries”) have been considered but are moot because the new ground of rejection does not rely on any reference applied in the prior rejection of record for any teaching or matter specifically challenged in the argument. Withdrawal of the previous ground of rejection has been necessitated by Applicant’s amendment filed 10/14/2025.
Conclusion
Applicant's amendment necessitated the new ground(s) of rejection presented in this Office action. Accordingly, THIS ACTION IS MADE FINAL. See MPEP § 706.07(a). Applicant is reminded of the extension of time policy as set forth in 37 CFR 1.136(a).
A shortened statutory period for reply to this final action is set to expire THREE MONTHS from the mailing date of this action. In the event a first reply is filed within TWO MONTHS of the mailing date of this final action and the advisory action is not mailed until after the end of the THREE-MONTH shortened statutory period, then the shortened statutory period will expire on the date the advisory action is mailed, and any nonprovisional extension fee (37 CFR 1.17(a)) pursuant to 37 CFR 1.136(a) will be calculated from the mailing date of the advisory action. In no event, however, will the statutory period for reply expire later than SIX MONTHS from the mailing date of this final action.
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/E.C./Examiner, Art Unit 1751
/JONATHAN G LEONG/Supervisory Patent Examiner, Art Unit 1751 2/9/2026